Chemical and Process Engineering 2013, 34 (1), 165-174

DOI: 10.2478/cpe-2013-0014

RESEARCH ON THERMAL DECOMPOSITION OF WASTE PE/PP

Monika Kuźnia*, Aneta Magdziarz

AGH University of Science & Technology, Faculty of Metals Engineering and Industrial Computer
Science , Al. Mickiewicza 30, 30-059 Krakow, Poland

The most important and the most frequently used plastics are polyethylene (PE) and polypropylene
(PP). They are characterised with high heating values (approximately 40 MJ/kg). Moreover, their
chemical composition, based mainly on carbon and hydrogen, allows to use them in industrial
processes. One of the methods of utilisation of plastic waste can be its use in the metallurgical
industry. This paper presents results of thermal decomposition of waste PE/PP. Chemical and
thermal analysis (TG) of studied wastes was carried out. Evolved gaseous products from the
decomposition of wastes were indentified using mass spectrometry (TG-MS). This paper also
presents an application of plastic wastes as supplemental fuel in blast furnace processes (as a
substitute for coke) and as an addition in processes of coking coal.
Keywords: plastic wastes, supplemental fuel, blast furnace process, coking of coal

1. INTRODUCTION

The growth in global steel production in 2001-2008 reached unprecedented amounts (Table 1). The
production of crude steel increased during this period by 497.7 million t, i.e. by 58.6%, and pig iron by
370 million t, i.e. by 64.2% (Kosewska and Merta, 2009). This increase was mainly generated by China
and India. The first symptoms of the economic crisis, which emerged in the fourth quarter of 2008,
forced steel manufacturers to reduce production amounts. However, it is only a matter of time before
the global economy comes out from recession.

Table 1. Crude steel production and blast furnace pig iron production in the world 2001-2008, mln t (Kosewska
and Mertas, 2009)

Year 2001 2002 2003 2004 2005 2006 2007 2008

Crude steel production 850.3 903.8 968.2 1054.7 1130.8 1250.0 1344.3 1329.7
Blast furnace production
578.5 611.1 658.5 717.8 788.9 868.8 946.3 927.1
of pig iron

Poland produced 9.7 million tonnes of crude steel in 2008, about 9% less than in the previous year. The
share of steel smelted in the Bessemer process accounted for 53.7%, and steel smelted in the electric
process – 46.3%. Poland belongs to the world's leaders in terms of the production of coke, used among
others in the blast furnace process. Table 2 below shows the largest producers of coke in the world.

At the same time, over the last several years there has been a steady increase in the production of
plastics. They are widely applied in many areas of life: as packaging, in construction, agriculture, the
automotive industry or in electronic equipment. Polyolefin, and particularly polyethylene and

*Corresponding author, e-mail: kuznia@agh.edu.pl

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polypropylene, account for 50% of all produced plastics. Their increasing production affects the
increase of the amount of waste generated and the need for its use. Besides material recycling, of which
the product is a recyclate for secondary production e.g. pots and garden furniture, chemical recycling is
also used - mainly for polyethylene terephthalate (PET) bottles. Material recycling is possible only after
the initial sorting of waste according to the types of plastic, and after removing impurities from them.
Both actions limit the profitability of material recycling of waste products. In addition, the ongoing
problem of segregation of municipal waste is responsible for the fact that a vast majority of such waste
is sent to a landfills, where it decomposes for even to a few hundred years. This waste can be
successfully used in the metallurgical industry. Plastic wastes can find application in the blast furnace
process as a substitute of coke (Kim et al., 2002; Fink, 1999) and as an additive in the coking of coal. In
the process of coke production, pyrolysis processes play a major role, whereas, in the blast furnace
process - combustion and gasification.

Table 2. Crude steel production and blast furnace pig iron production in the world 2001-2008, mln t (Kosewska
and Mertas, 2009)

Country 2007 2008

China 328.80 322.01
Japan 38.30 39.50
Russia 31.90 30.00
India 19.40 22.50
Ukraine 19.60 19.00
USA 15.00 14.80
South Korea 10.00 11.50
Poland 10.30 9.83
Brazil 8.60 9.50
Germany 8.50 9.20

The main sources of obtaining plastic waste include (Niesler, 2001):

• municipal waste,
• unutilised post-production waste,
• recycling of cars.

In recent years, remains from the process of automobile shredding, containing not only scrap metal, but
also more and more plastic, have found application in blast furnace processes (Mirabile et al., 2002).
Plastic recovered from shredded automobiles is very diverse in terms of assortment (more than 20
types) and contaminated. Therefore, the possibilities of its use in material recycling are very limited.
Used electronic equipment also finds application in the blast furnace process.

2. DISPOSAL OF PLASTIC WASTE

There are two methods of disposal of plastic waste in metallurgical processes. The first is utilisation of
plastic waste in the blast furnace process. During this process plastic waste generates a lot of flammable
gases, which are a precious fuel in blast furnace process. The second use of plastic waste is using it in
the coking process (CARBOTHERM process). During this process plastic wastes are destroyed by the
coke formation process. An addition of plastic waste during the coke formation process does not
adversely affect it.

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2.1. Application of plastic waste in the blast furnace process

Providing a blast furnace with plastic waste first begun in foundries in Germany and Japan in 1995
(Maki and Ariyama, 2003; Okuwaki, 2004). German steel manufacturers: Stahlwerke Bremen and
Krupp Hoesch substitute fuel oil, used in the production of pig iron, with granular plastic. Industrial
and municipal plastic waste is used, which does not meet the conditions for material recycling. These
two German steelworks use up to 30% of fuel oil used in the production process of pig iron in blast
furnaces with plastic. In Japan plastic waste in the blast furnace process began to be used more or less
at the same time as in Germany. In the blast furnaces, the only egzothermal reaction is the combustion
of coke and substitute fuel. Generated heat is necessary to reduce iron oxides and melts created iron.
Depending on the ironworks, fuel oil or coke is replaced with plastics in the amount of several dozen
kilograms per tonne of crude steel. This method provides considerable savings, on the one hand, by
reducing the purchase of expensive coke, and on the other hand, by not having to pay for the collection
of waste.

Thin, lightweight foil is broken down, melted and granulated; granules that are produced are sent to a
silo. Large, solid waste is first crushed in a two-step process; then granulated. The final product is sent
by a conveyor pipe to the same silo. From there, they go to a container of a blower, which then blows
them through nozzles into a blast furnace. Granules of a diameter of 6-10 mm are fed into a blast
furnace by a device that also injects pulverised coal (PCI-pulverized coal injection) through nozzles.
Hot air is injected into the bottom of the furnace at high speed, creating a combustion zone, in which
plastics are subject to gasification (incomplete combustion) to CO and H2. While pulverised coal or
coke quickly undergo combustion immediately after entering the zone of oxidation, using up O2 and
generating CO2 at a temperature above 2000 °C (Ogaki et al., 2001):
C + O 2 → CO 2 (1)

In the final combustion zone, once all the oxygen is consumed, CO is created as a result of the reaction
of CO2 with coke:
C + CO 2 → 2CO (2)

Plastic exposed to CO2 degrade into CO and H2 (as an example in the reaction polyethylene was used):
1
C 2 H 4 + CO 2 → 2CO + H 2 (3)
2

Hydrogen resulting in the process of degradation of plastic is a reducer in the blast furnace acting
jointly with CO. The reaction of reduction with H2 is less endothermal than a direct reaction with C,
which is of course beneficial for the heat balance of the blast furnace. The reaction of reduction of iron
oxides proceeds as follows:
Fe 2 O 3 + 3CO → 2Fe + 3CO 2 (coke, plastic wastes) (4)

Fe2O3 + 2CO+ H2 → 2Fe + 2CO2 + H2O (plastic wastes) (5)

Applying plastic waste reduces CO2 produced in the blast furnace process by approx. 30% compared to
using only coke and pulverised coal. In addition, resulting gases, which are recovered at the exit of a
blast furnace, are enriched in hydrocarbons produced from the decomposition of plastic, have a high
calorific value. In Poland, a significant part of generated plastic waste can also be utilised in blast
furnaces. However, the cost of adapting nozzles providing air to delivering plastic wastes granules is a
large barrier. Another method of recycling plastic waste in blast furnaces is their direct input in the
blast furnace feedstock. This method would enable to use plastic waste almost without any investments.
Slight financial outlay would be connected only to the process of grinding or granulating of
polyethylene foils. In Poland, at the Institute of Iron Metallurgy, studies are being carried out on

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utilising plastic waste in blast furnaces (Niesler, 2001; Niesler and Stecko, 2000). Industrial trials were
carried out with the addition of waste in quantities of about 7 kg/t of pig iron, for a period of 12 days.
Applying plastic waste not containing silica of carbon content approx. 78% and hydrogen approx. 12%,
affects the economy of coke in the blast furnace process. However, the use of waste containing glass
fibres with a high content of silica can have an impact on increasing the share of raw flux in the
feedstock and on an increase in the consumption of coke associated with this. Chlorine content in blast
furnace dust was approximately 0.6%. This is not a value exceeding the limits of chlorine content in
blast-furnace dust, which is approximately 0.3-0.75%. Due to the possibility of dioxin formation and
the corrosive properties of chlorine compounds arising from the degradation of polyvinyl chloride
(PVC) should be removed from the waste stream fed into a blast furnace. The limit of chlorine content
in raw material should not exceed 1% by weight. For waste with a high content of chlorine - gas
treatment installations must be based on chemical absorption and catalytic or adsorption treatment and
devices of blast furnace should be made of materials with high resistance to corrosion. In order to use
waste with a high chlorine content (more than 2%), a dechlorifying technology developed in Japan can
be used. It consists in heating raw materials containing chlorine at a temperature of 300-400°C, in an
oxygen-free atmosphere. These raw materials are subject to thermal decomposition with a release of
hydrogen chloride. The substance that has been dehydrochlorinated, after cooling and granulating, can
be used in a blast furnace. Hydrogen chloride is absorbed in water, refined by distillation and recycled
as hydrochloric acid (HCl). Owing to high construction costs of a dehydrochlorination station PVC is
most often removed from the waste stream fed into a blast furnace.

2.2. Applying plastic waste in the coking process

Waste plastic can be used directly in coke chambers, where at high temperatures, together with coal, it
is subject to thermal decomposition to: coke (20%), oils (40%) and coke gas (40%) (Nomura et al.,
2003; Okuwaki, 2004).

2.2.1. Direct addition to the coke feedstock

An addition of plastic waste at the level of 1% to coke coal does not cause changes to the properties of
coke (Niesler, 2001). Adding plastic at the level of 2%, containing aliphatic polymers such as:
polyethylene (PE), polypropylene (PP) and polyvinyl chloride (PVC) has only a minor impact on the
deterioration of coke's durability. In some cases, the addition of polyethylene even caused an increase
in coke's durability. Figure 1 shows the effect of plastic addition on coke strength. Coke drum strength
increases slightly in the case of PE addition, but the addition of PS and PET decreases coke drum
strength to a great extent. The drum strength of PET addition coke is lower than that of PS addition
coke because PET addition decreases the coal caking property more than PS addition. Figure 2 shows
the effect of the addition of plastic waste on the index CRI (coke reactivity index). The addition of
plastic to coal, in all cases, causes CRI to rise. This is due to the increase in the porosity of coke in all
cases for which the addition of plastic waste was used (Figure 3). The cause of this phenomenon is the
emergence of empty spaces in coke, resulting from the thermal process of decomposition of plastic
particles. Figure 4 shows the influence of the plastic waste addition on CSR (coke strength after
reaction). In the case of applying polyethylene an increase in CSR has been observed. This is caused by
the growth of DI (Dilatation Index). For PS and PET addition, CSR decreases due to both a lower DI
and a growth of CRI. The impact of plastic waste on the properties of coke is different depending on
the material used. These differences are caused by the mutual effects between thermal products of
plastic waste degradation and hydrogen from coal. Radicals resulting from the thermal process of
degradation of PS and PET remove hydrogen from carbon, which may result in the deterioration of
properties of coals of carbon. PE shows a trend of "transferring" hydrogen from plastic to carbon
(Nomura, 2003). A direct addition of plastic waste to the coke feedstock has been used widely in Japan.

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Since 2000, in Japan, in coking plants in Nagoya and Kimitsu, and since 2002 in coke plants in Yahata
and Muroran, plastic waste has been dosed into the coke feedstock. The size of the addition amounts to
1%, which allows to dispose of 140 000 Mg plastic waste/year. Attempts are also being made do
directly dose plastic waste (up to 3%) to the coke feedstock in Ukraine. Studies on the application of
direct addition are also being conducted in China.

90 30 PET
Coal PE PS
80 PS PET PE
Coal
25
70

60 20
DI15015 [-]

50

CRI [-]
15
40

30 10

20
5
10

0 0

Fig. 1. Effect of plastic addition on coke strength Fig. 2. Effect of plastic addition on CRI
(Nomura et al., 2003) (Nomura et al., 2003)

50 PET 70
PE PS Coal PE
Coal
PS
60 PET
40
50
Porosity [%]

30 40
CSR [-]

30
20

20

10
10

0 0

Fig. 3. Effect of plastic addition on porosity Fig. 4. Effect of plastic addition on CSR
(Nomura et al., 2003) (Nomura et al., 2003)

2.2.2. Application of the CARBOTHERM process

A direct addition of split plastic waste to carbon mixture, in theory the simplest way of their use in the
coke industry, is limited by a number of phenomena. This solution affects negatively the quality of
coke (increased reactivity and reduced strength), as well as technological process (excessive degassing
in the first phase of coking causing increased pressure in the coke chamber). Additionally, due to the
formation of hydrogen chloride, it is necessary to separate PVC from the waste stream. These problems
can be eliminated through the application of the CARBOTHERM process of plastic waste combined
with partial degassing and structural destruction of polymers (thermolysis). The method was developed
jointly by the Institute of Chemical Processing of Coal in Zabrze, Poland, and the Institute of Industrial
Chemistry in Warsaw (Kijeński and Polaczek, 2005; Sobolewski and Wasilewski, 1998; Sobolewski

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and Wasilewski, 2005). The CARBOTHERM process (Figure 5) leads to obtaining a component of the
carbon feedstock of full value for the coking industry. This allows to both carry out the process of deep
dechlorinating of plastic waste, and eliminate technological difficulties concerned with the process of
cooling and solidification of the product of plastic waste thermopreparation. Carbotherm process also
bypasses the operation of its grinding to a particle size that is compatible with technological
requirements of the process of coking coal. In order to bring the physico-chemical properties of
processed waste closer to the coal mixture, plastic waste is subjected to the process of
thermopreparation.

Plastic wastes Coal-tar pitch

Homogenisation
t = 250 °C
Adsorption of hydrogen
chloride and Hydrochloric acid
combustion of gas
Thermolysis
t = 350 °C
Cooling vapours
Hard coal

Non-diaphragm cooling of liquid thermolysis CARBOTHERM

products

Fig. 5. Block diagram of CARBOTHERM technology (Sobolewski and Wasilewski, 2005)

Plastic waste generated from the entire stream of municipal waste, after mechanical reduction, is
subjected to the two-stage process of thermolysis in coal or petroleum bitumen. To this end, plastic
waste is mixed with hot, liquid coal-tar pitch the recommended mass ratio plastic waste/bitumen = 4/1,
not exceeding the temperature of 250°C, without extracting volatile products. After initial
homogenisation, the substrates are heated in the thermolysis reactor up to the temperature of 350 °C
and are subjected to shear stress, which breaks causes the breaking of polymer chains (Sobolewski and
Wasilewski, 2006). Small quantities of raw gas extracted during this process is subject to treatment
from hydrogen chloride (originating from the decomposition of polyvinyl chloride). After the
absorption of hydrogen chloride, raw gas combusts, and the resulting heat is used to conduct the
thermolysis process. The hot, liquid product of thermolysis is mixed with culm, causing its cooling and
solidification on the surface of coal grains. The resulting solid product which has been called
CARBOTHERM - is loose, thermomechanically stable, and does not change its properties during
storage. It can constitute both a coal feedstock for coking, and a substitute for solid fuel with a higher
calorific value. In Table 3 a comparison is shown of the physico-chemical properties of hard coal and
the finished product CARBOTHERM. The results of the analyses indicate a very large similarity of the
properties of hard coal and CARBOTHERM.

First laboratory tests and then industrial tests were carried out in the Coking Plants "Wałbrzysz" S.A.
(Wasilewski and Sobolewski, 1998). Below (Table 4) the properties of coke obtained in industrial tests
are shown. In assessing the results of determination of coke, it can be claimed that an addition of 5% of
a thermolysis product to a coal mixture did not have a great influence on the parameters of coke
strength nor on its reactivity (all results are within the limits of determination error). The chlorine
content in coke produced from the coke mixture with the addition of a thermolysis product increased
slightly, without exceeding the value normally obtained in classic coke.

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Table 3. Physical and chemical properties of coal and CARBOTHERM product (Sobolewski and Wasilewski,
2005)

Parameter Hard coal CARBOTHERM

Elemental analysis, wt. %
C 84 83.05
H 7 7.95
O 7.9 7.92
N 0.4 0.34
S 0.5 0.45
Cl 0.2 0.21
3
Bulk density, kg/m 850 900
Calorific value, MJ/kg 27 33
Mechanical properties brittle Brittle

Table 4. Properties of cokes obtained in the industrial tests (Wasilewski and Sobolewski, 1998)

First industrial tests Second industrial tests

Parameter addition of 5% addition of 5%
coal mixture of a thermolysis coal mixture of a thermolysis
product product
Aa, wt. % 11.8 11.8 11.8 11.8
a
Cl , wt. % 0.2 0.236 0.2 0.236
CRI, % 52.5 49.2 52.5 49.2
CRS, % 29 33.8 29 33.8
Coke strength, % 83.7 83.5 83.7 83.5

3. EXPERIMENTAL

In order to determine the suitability of plastic waste for use in blast furnace process it is necessary to
carry out a series of studies, among others, in the scope of elemental analysis, the process of thermal
decomposition or analysis of chemicals produced in the process of decomposition. The results are very
important for blast furnace technology. Especially the composition of gases generated in the process of
thermal decomposition is significant for DRI (Direct-reduced iron) process. In this work the results of
the thermal analysis are presented.

3.1. Materials

Three samples of plastic waste from a polyolefin group were studied: 2 samples came from packaging
for cosmetics and cleaning products containing high density polyethylene (PE-HD) and polypropylene
(PP), the third sample came from the agricultural and horticultural industries and this sample was used
for covering tunnels containing low density polyethylene (PE-LD).

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3.2. Instrumental methods

For test samples an elemental analysis was conducted - the chemical composition, ash content and
calorific value were examined. The elemental analysis was carried out by the elemental analyser Leco
SC 132 and Leco CR 12. The calorific value was calculated on the basis of measurements made using
a calorimeric bomb.

Thermogravimetric analysis is one of the instrumental methods used to analyse plastic wastes. In the
present study thermogravimetry (TG) was carried out on the tested samples. Thermogravimetric
analysis was carried out using a Mettler Toledo TGA/SDTA 851e apparatus. The TGA instrument was
calibrated with indium, zinc and aluminium. Its accuracy was equal to 10−6 g. For the
thermogravimetric analysis (TG) the samples were placed in alumina crucible. C.a. 2 mg of the sample
was heated from an ambient temperature up to 1000°C at a constant rate: 10 °C/min in 3 dm3/h flow of
air. The measurements for each sample had to be done under exactly the same conditions including e.g.
the range of temperature, atmosphere, heating rate, etc. to determine the most repeatable and precise
results. The experiments were replicated to determine their reproducibility, which was found to be very
good. TG curves for each fuel sample were obtained as an output. TG curves were used in order to
assess the thermal characteristics of plastic waste.

Evolved gaseous products from the decomposition of studied samples were identified on-line, using
connected to ThermoStar GSD300T Balzers quadruple mass spectrometer (QMS). The mass
spectrometer was operated in electron impact mode (EI) using channeltron as a detector. Screening
analyses were performed in the selected-ion monitoring (SIM) mode. The following ion characteristic
of each molecule, such as: 16, 18, 28, 29, 39, 40, 41, 43, 44 and 78 for CH4, H2O, C2H6, C3H8, C4H6,
C3H4, C3H6, C4H10, CO2 and C6H6. were monitored. It is important to notice that the QMS spectrum of
mass 28 can represent not only C2H6 but also C2H4 , and 29 can represent also CH2O and C2H4O.

4. RESULTS AND DISCUSSION

The results of the elemental analysis indicate clearly a very similar chemical composition of the tested
materials (Table 5). The carbon content in the analysed waste (82.8-83.1%) is very high, while the
sulphur content in the materials (0.03-0.1%) is low, which has a substantial impact on reducing
emissions of SOx. It is worth noting a very low ash content and a very high calorific value of the tested
samples, which significantly raises the value of the waste used as fuel in the blast furnace process.

Table 5. Elemental analysis of polyolefine wastes

PE-LD PE-HD PP
Elemental analysis, wt. %
H 14.93 15.1 15.26
C 82.8 83 83.1
S 0.07 0.1 0.03
N 1.93 1.21 1.46
Ash, wt. % 0.01 0.7 0.06
Calorific value, MJ/kg 42.23 42.78 43.34

On the basis of the results of the TG-MS analysis both the process of thermal decomposition (TG
curves) was conducted and the presence of chemical compounds in waste gases, depending on the

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temperature was determined. The shapes of TG curves are very similar, and the residue after
incineration is very small (Figure 6). Thermal decomposition begins at a temperature of approx. 250 °C
and ends at approx. 550 °C, except the temperature at the end of decomposition of polypropylene,
which is appox. 400 °C. It is easy to notice that the maximum speed of the decomposition of
polyethylene takes place at a temperature of approx. 400 °C, while that of polypropylene at approx.
300 °C. The beginning of the process of decomposition can be caused by the combustion of compounds
from an alkanes group, whose temperature of spontaneous combustion is lower than 250 °C
(e.g. n-hexane and n-heptane, n-octane, n-nonane, n-decane, n-undecane). These compounds are
products of the main chain of polymer splitting, therefore, they arise in relatively low temperatures
(they do not require a large amount of energy to a possible recombination). Further stages in the
process of decomposition are associated with the process of compound combustion, which includes: n-
butane, 1,3-butadiene, ethane and ethylene, and these gases occur at a temperature of approx. 350 °C,
400 °C and 450 °C. Mass spectrometry analysis also revealed the presence of combustible compounds
with higher (than 450 °C) ignition temperature such as: CH4, CO and C6H6. During the identification of
certain chemical compounds the database of NIST (National Institute of Standards and Technology)
was used.

100

80
Mass change [%]

60

40

PE-HD
20 PP
PE-LD

0
100 200 300 400 500 600
Temperature [oC]

Fig. 6. TG curves for PP, PE-HD and PE-LD

Both chemical composition (high content of carbon and hydrogen), high calorific value and the
composition of gases generated in the process of decomposition, make the tested polyolefin waste
constitute a valuable substitute for coke in the blast furnace process. Feeding waste together with a
feedstock generate gases educed in the thermal process of decomposition. In addition, hydrocarbons
generated in the first phase of decomposition increase the calorific value of the blast-furnace gas. Due
to a very similar composition of hard coal used in the coking process (Table 3), polyolefin waste can be
used as an additive in coking coal.

5. CONCLUSIONS

One of the methods of utilisation of plastic waste can be its use in the metallurgical industry. This
waste is used as a substitute for coke in the blast-furnace process or as an additive to coal in the coking
process. In blast furnace process plastic waste can be fed via nozzles supplying air, at the bottom of a
furnace or at the top together with the feedstock. In the coking process an addition of plastic can be
applied directly to the coke feedstock (this method, however, has many defects) or after a prior
completion of the process of CARBOTHERM (thermopreparation). In order to determine the suitability

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of different groups of plastic to the above mentioned processes, it is necessary to carry out a series of
tests of thermal analysis. Due to the chemical composition and the quality of the products generated in
the process of thermal decomposition (n-hexane and n-heptane, n-octane, n-nonane, n-decane, n-
undecane, n-butane, 1,3-butadiene, ethane, ethylene, CH4, CO and C6H6), waste from the polyolefin
group constitutes a very attractive group of materials used in blast furnace process. CO from the
thermal decomposition of waste is both a fuel and a reducer. However, hydrocarbons produced in
decomposition processes significantly increase the calorific value of the gas furnace.

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Received 23 April 2012

Received in revised form 11 February 2013
Accepted 14 February 2013

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